Alleviation Of Laser-Induced Damage In Optical Materials By Suppression Of Transient Color Centers Formation And Control Of Phonon Population

ABSTRACT

Laser-induced damage in an optical material can be mitigated by creating conditions at which light absorption is minimized. Specifically, electrons populating defect energy levels of a band gap in an optical material can be promoted to the conduction band—a process commonly referred to as bleaching. Such bleaching can be accomplished using a predetermined wavelength that ensures minimum energy deposition into the material, ideally promoting electron to just inside the conduction band. In some cases phonon (i.e. thermal) excitation can also be used to achieve higher depopulation rates. In one embodiment, a bleaching light beam having a wavelength longer than that of the laser beam can be combined with the laser beam to depopulate the defect energy levels in the band gap. The bleaching light beam can be propagated in the same direction or intersect the laser beam.

RELATED APPLICATIONS

This application claims priority of U.S. Provisional Patent Application61/292,375, entitled “Alleviation Of Laser-Induced Damage In OpticalMaterials By Suppression Of Transient Color Centers Formation AndControl Of Phonon Population” filed Jan. 5, 2010.

BACKGROUND OF THE INVENTION

1. Field of the Invention

The present invention relates to laser systems and in particular tominimizing damage to optical materials, such as crystals, that are usedin laser systems.

2. Related Art

Optical materials are key elements of modern-day laser systems. Commonapplications for optical materials include fabrication of basic opticalcomponents (e.g. windows, mirrors, polarizers, etc.) as well asnonlinear optical devices for frequency mixing (e.g. harmonicgeneration, parametric generation/amplification), Raman amplification,Kerr-lens modelocking, electro-optic modulation, and acousto-opticmodulation.

When exposed to laser radiation, physical properties of these opticalmaterials may change with time as a result of interaction between lightand matter. Such changes may adversely affect optical propertiesincluding, but not limited to, transmittance, reflectivity, andrefraction indices. These adverse changes are generally referred to asmaterial damage. The material lifetime, i.e. the amount of time in whichthe material is serviceable for its intended purpose within a range ofaccuracy, is typically defined based on a maximum acceptable change inone or more of these parameters.

Laser-induced damage of optical materials is one of the main factorsaffecting material lifetime, thereby limiting performance of lasersystems. Laser-induced damage has been subject to extensive research,which has focused on (i) improving the quality of the existing opticalmaterials and development of new compounds that possess high laserdamage tolerance and/or (ii) optimization of operating conditions tomitigate laser-induced damage. This optimization of operating conditionshas become increasingly important as the growing demand for high powerDUV (deep ultraviolet light having a wavelength λ <300 nm) lasersimposes such extreme material requirements that conventional damagetolerance improvement approaches quickly become insufficient, toocostly, and/or impractical.

The most common technique used to mitigate laser-induced damage isthermal annealing. It is widely employed as a method of reducinglaser-induced damage because it works for many different types of damagein various materials and is relatively easy to implement. Unfortunately,efficient thermal annealing can require a high temperature, which whenused during real-time laser system operation can pose significantdisadvantages.

First, presence of a high temperature inside a laser system is highlyundesirable because thermal gradients can cause air fluctuations thatresult in output beam instability and increased outgassing intensifiesphotocontamination. Second, at short (e.g. DUV) wavelengths, when photonenergies approach band gaps of common optical materials, phonon-assistedabsorption becomes significant and increases exponentially withtemperature. This absorption can lead to decline in overall systemperformance, for example, one can observe decreased conversionefficiency when applied to nonlinear frequency conversion. Moreover,this phonon-assisted absorption may exacerbate other laser-induceddamage to the optical material, thereby potentially negating thepositive effects of annealing.

Note that in certain situations, the temperature of the optical materialneeds to be precisely controlled for reasons unrelated to materiallifetime. For example, in non-critical phase matching (for certainwavelengths combinations only), the phase mismatch can be minimized byadjusting the crystal temperature such that the phase velocities of theinteracting beams are equal. Therefore, for such situations, theapplication of thermal annealing is limited, if at all possible.

Therefore, a need arises for a technique of minimizing laser-induceddamage in optical materials that overcomes the drawbacks of conventionalannealing.

SUMMARY OF THE INVENTION

Damage can occur when light energy is deposited into an optical materialvia light absorption. As described in further detail herein with respectto the present invention, laser-induced damage in an optical materialcan be mitigated by creating conditions at which light absorption isminimized. Specifically, electrons populating defect energy levels of aband gap in an optical material can be promoted to the conduction band—aprocess commonly referred to as bleaching. Such bleaching can beaccomplished using a predetermined wavelength that ensures minimumenergy deposition into the material, ideally promoting electrons to justinside the conduction band. In some cases phonon (i.e. thermal)excitation can also be used to achieve higher depopulation rates.

In one embodiment, a bleaching light beam having a wavelength longerthan that of the laser beam can be combined with the laser beam todepopulate the defect energy levels in the band gap. The bleaching lightbeam can be propagated in the same direction or intersect the laserbeam. In one embodiment to optimize depopulation, both the bleachinglight beam and the laser beam can be pulsed with a delay between thepulses of the two sources, i.e. the bleaching light beam and the laserbeam. In another embodiment, one wavelength of a laser beam havingmultiple wavelengths can be delayed and propagated with the laser beam,thereby also depopulating the defect energy level.

In one embodiment using a pulsed laser, the temperature of the opticalmaterial can be modulated such that it is low during the laser pulse andhigh between the pulses and/or when no laser pulses propagate throughthe optical material. The advantage of temperature modulation is moreefficient thermal annealing of defects when no laser pulses are presentwithout increase in light absorption due to high temperature. In anotherembodiment, a temperature gradient can be created inside the opticalmaterial and varied in time such that a laser beam always propagatesinside the lower-temperature region while the higher-temperature part ofthe optical material undergoes intense annealing. At a later point intime, the temperature distribution inside the optical material can bemodified such that the temperature of the previously “hot” regions islowered and the laser beam can be shifted to those regions while thetemperature of the previously “cold” region is raised. Thus, atime-dependent temperature gradient can be created inside the opticalmaterial. This cycle can be repeated multiple times.

Note that this temperature adjustment can be performed in combinationwith the above-described optical excitation or separately. Theabove-described techniques can eliminate maintaining the opticalmaterial at high temperature, thereby avoiding the conventional inherentdisadvantages of annealing. Therefore, these localized annealingtechniques can provide increased applicability in cases whereconventional material temperature adjustment is impossible (such as incase of non-critical phase matching) or impractical.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 shows one mechanism of transient color center formation.

FIG. 2 illustrates examples of light absorption processes in whichphoton energy is smaller than the band gap E_(gap) of the opticalmaterial, thereby prohibiting direct excitation from a valence band to aconduction band.

FIG. 3 shows a preferred mechanism of transient color center relaxation.

FIG. 4 illustrates an exemplary laser system including a laser lightsource, a bleaching light source, and a beam combiner.

FIG. 5 illustrates an exemplary laser system including a laser lightsource, a focusing lens, and a bleaching light source.

FIG. 6A illustrates an exemplary technique using a pump pulse associatedwith a pulsed laser beam and a probe pulse associated with a pulsedbleaching light source, wherein the two pulses are separated by apump-probe delay.

FIG. 6B illustrates experimental data of 532 nm absorption dependence onthe delay between 193 nm and 532 nm pulses in CLBO crystal.

FIG. 7 illustrates a laser system in which an optical delay element canprovide an optical delay for one wavelength of laser light source beforethe laser light (of multiple frequencies) passes through the opticalmaterial.

FIGS. 8A and 8B illustrate a technique of performing efficient thermalannealing by creating a temperature gradient inside the optical materialand varying it in time such that a laser beam always propagates insidethe lower-temperature region while the higher-temperature part of theoptical material undergoes intense annealing.

FIG. 9 illustrates results of temperature optimization to maximizelifetime of a non-linear CLBO crystal under exposure to 193.3 nmradiation.

DETAILED DESCRIPTION OF THE DRAWINGS

During light absorption by an optical material, electrons are promotedfrom a valence band, which is a low energy state, to a conduction band,which is a high energy state. Electrons promoted to the conduction bandmay spontaneously lose energy and then return to the valence band in aprocess that releases energy in the form of light, i.e. fluorescence.Electrons that are too energetic (i.e. extend far into the conductionband) can cause significant damage to the material. That is, suchelectrons in the conduction band are “free” (i.e. non-bound) electronsthat can move freely, accelerate, and release considerable amounts ofenergy (e.g. enough to break bonds of the crystal) before fluorescencetakes place.

FIG. 1 shows one mechanism of transient color center formation. In stepA, an initial absorption promotes an electron e from a valence band 101to a conduction band 102. In an ideal crystal, a band gap is spaced tohave no intermediate energy levels between valence band 101 andconduction band 102. Therefore, in an ideal crystal, no electrons wouldend up inside the band gap. An actual crystal generally has one or moreisolated energy levels present in the band gap, typically close toconduction band 102. FIG. 1 shows one such defect energy level 104formed in the band gap.

In step B, an energy transfer (i.e. loss) results in a population ofdefect energy level 104 inside energy band gap E_(gap). That is, one ormore electrons, instead of returning to valence band 101, populatedefect energy level 104. This population of defect energy level 104 isalso called a transient color center because the electrons populatingdefect energy level 104 can begin to absorb wavelengths not previouslyabsorbed, thereby resulting in a temporary change in absorption spectrumof the optical material.

For electrons populating defect energy level 104, some electrons maylose energy and return to valence band 101 and other electrons may gainenergy via a secondary light absorption 103 and be promoted toconduction band 102 in step C. Unfortunately, any electrons deep inconduction band 102 (which can easily occur because of the energyassociated with secondary light absorption 103) can result in increaseddamage to the optical material, as described above.

FIG. 2 illustrates examples of light absorption processes in whichphoton energy (as represented by the length of an arrow) is smaller thanthe band gap E_(gap) of the optical material, thereby prohibiting directexcitation from a valence band 210 to a conduction band 211. In FIG. 2,λ₃<λ₁<λ₂ (i.e. the wavelength is inversely related to the length of thearrow). Notably, a photon having a wavelength λ₃ has more energy than aphoton having a wavelengths λ₂ or λ₁.

In FIG. 2, process 201 is a single-color two-photon absorption, which isshown by two arrows. Each arrow represents a photon having a wavelengthλ₁. Process 202 is single-color three-photon absorption, which is shownby three arrows. Each arrow represents a photon having a wavelength λ₂.Process 203 is multi-color two-photon absorption, which is shown by twoarrows. A first arrow represents a photon having a wavelength λ₁,whereas a second arrow represents a photon having a wavelength λ₂.

Process 204 is phonon-assisted absorption in which a single photonhaving a wavelength λ₃ (which is close to but less than the band gapenergy E_(gap)) is absorbed simultaneously with the phonon (a quantum ofa material's internal vibration). Note that because phonons obeyBose-Einstein statistics, their population increases exponentially withtemperature and so does the probability of phonon-assisted absorption.

FIG. 3 shows a preferred mechanism of transient color center relaxation.Specifically, in step D, the promotion of electrons from defect energylevel 104 into conduction band 102 can be accomplished with the leastamount of energy absorption, i.e. just reaching into conduction band102. Subsequently, in step E, electrons can quickly return to valenceband 101 via emission of a photon (fluorescence) or another mechanism,while minimizing the possibility of damage to the material.Specifically, the amount of energy deposited into the optical materialis minimized, thereby reducing laser-induced damage rate and increasingoptical material lifetime.

The above-mentioned promotion of electrons from defect energy level intothe conduction band can be achieved by using low energy optical and/ornon-optical excitations (i.e. used separately or in combination). Theoptical excitation, i.e. bleaching, needs to be performed at awavelength λ_(b) that satisfies two conditions:

$\begin{matrix}{{i.\mspace{14mu} \frac{\; {hc}\;}{\lambda_{b}}} \geq E_{def}} & (1) \\{{i\; {i.\mspace{14mu} \lambda_{b}}}\operatorname{>>}\lambda_{1}} & (2)\end{matrix}$

where h is Planck's constant, c is the speed of light, E_(def) is theminimum energy required to excite an electron from defect energy level104 to conduction band 102 (see FIG. 3), and λ₁ is the laser wavelengththat causes most of the optical material damage (typically the shortestwavelength). In one embodiment, to meet condition (2), at least a factorof 3 may be used. Note that for non-optical excitation in step D,phonons (described above) can be used. However, their population must becontrolled such that phonon-assisted absorption of original laser lightdoes not take place, which in many cases places restriction on thetemperature of the optical material.

FIG. 4 illustrates an exemplary laser system 400 including a laser lightsource 401, a bleaching light source 402, and a beam combiner 403.Bleaching light source 402 emits a light beam having a wavelength λ_(b),which, when combined and co-propagated with a laser beam from laserlight source 401 having one or more wavelengths λ₁, λ₂, . . . , λ_(N)using beam combiner 403, can maximize efficient depopulation of thedefect energy levels associated with optical material 404. (Note thatwhether the laser beam includes one wavelength or multiple wavelengthsλ₁, λ₂, . . . , λ_(N), conditions (1) and (2) must hold true withrespect to wavelength λ_(b).) In one embodiment, a temperaturecontrolled environment 405 can be used to control phonon populationinside optical material 404. Note that this optical bleaching andtemperature control can be used separately or combined, depending onwhat is best suited for a particular laser system and its application.

FIG. 5 illustrates an exemplary laser system 500 including a laser lightsource 501, a focusing lens 502, and a bleaching light source 503.Bleaching light source 503 emits a radiation λ_(b) that can be combinedwith the radiation λ₁, λ₂, . . . , λ_(N) emitted from laser light source501 (and focused by lens 502) to maximize efficient depopulation of thedefect energy levels associated with optical material 504. In this case,the co-propagation of the bleaching radiation is not necessary becauseonly a small volume inside optical material 504 close to the focal planeis exposed to high laser fluence. Thus, this small region can bebleached locally by propagating the bleaching light at an angle (e.g.90°, perpendicular to, or at some other intersecting angle) to theoriginal laser beam, thereby providing a simple configuration for lasersystem 500. In one embodiment, a temperature controlled environment 505can be used to control phonon population inside optical material 504.Once again, this optical bleaching and temperature control can be usedseparately or combined, depending on what is best suited for aparticular laser system and its application.

If laser light sources 401 and 501 (FIGS. 4 and 5, respectively) arepulsed, then bleaching light sources 402 and 503 can also be pulsed andshifted in time with respect to those of the laser source. For example,FIG. 6A illustrates an exemplary technique using a pump pulse 601associated with a pulsed laser beam and a probe pulse 602 associatedwith a pulsed bleaching light source, wherein pulses 601 and 602 areseparated by a pump-probe delay 603. Advantageously, by minimizing thetemporal overlap between the two light sources, cross-absorption (i.e.process 203 in FIG. 2) can be minimized. An electron at a defect energylevel would preferably receive another photon at λ₂ (which wouldfacilitate step D, FIG. 3) rather than another photon at λ₁ (which couldresult in step C, FIG. 1).

Exemplary bleaching of transient color centers with λ_(b) satisfyingconditions (1) and (2) can include an ArF (argon fluoride) excimer (193nm) and frequency doubled Q-switched Nd:YAG (neodymium-doped yttriumaluminium garnet) (532 nm) lasers in a pump-probe configuration toobserve absorption of 532 nm light induced by 193 nm light inside aCesium Lithium Borate (CLBO) non-linear crystal (a non-linear opticalmaterial used to obtain DUV radiation by non-linear frequency conversionof solid-state and fiber laser infrared outputs).

FIG. 6B illustrates experimental data 606 of 532 nm absorptiondependence on the delay between 193 nm and 532 nm pulses. Note that data606 supports evidence that the induced 532 nm absorption is caused bytransient species, i.e. transient color centers, because the amount ofabsorption (which is proportional to color center concentration) decaysas function of pump-probe delay. Data 606 further supports evidence thatlonger wavelength light (e.g. 532 nm or similar wavelengths) can be usedto effectively bleach these transient color centers, thereby preventingsecondary absorption of original light (e.g. 193 nm or similarwavelengths) that would deposit much larger amounts of energy into theoptical material.

Notably, each optical material may have an optimized delay between laserand bleaching light pulses to ensure cross-absorption minimization aswell as transient color center bleaching maximization.

Note that when multiple wavelengths are present in the laser system,such as in the case of non-linear frequency conversion, it may bepossible to use one of the wavelengths as a bleaching radiation as longas it satisfies conditions (1) and (2) discussed above. For frequencyconversion process, for example, such wavelength could be a fundamentalwavelength or one of the lower harmonics. As with the case of a separatebleaching light source, a temporal shift of the bleaching light isdesirable and can be achieved by placing an optical delay element todelay light of a certain wavelength with respect to other wavelengths.For example, FIG. 7 illustrates a laser system 700 in which an opticaldelay element 702 can provide an optical delay for one wavelength oflaser light source 701 before the laser light (of multiple frequencies)passes through optical material 703. In one embodiment, atemperature-controlled environment 704 can also be used to controlphonon population inside optical material 703.

In one embodiment using a pulsed laser, the temperature of the opticalmaterial can be modulated such that it is low during the laser pulse andhigh between the pulses and/or when no laser pulses propagate throughthe optical material. The advantage of temperature modulation is moreefficient thermal annealing of defects when no laser pulses are presentwithout increase in light absorption due to high temperature.

FIGS. 8A and 8B illustrate a technique of performing efficient thermalannealing by creating a temperature gradient inside the optical materialand varying it in time such that a laser beam always propagates insidethe lower-temperature region while the higher-temperature part of theoptical material undergoes intense annealing. For example, at time 801(FIG. 8A), a laser beam can shift from left to right in alower-temperature region of optical material 810 (shown in crosssection) while a higher-temperature region undergoes thermal annealing(shown as the bottom region). At a later point in time, the temperaturedistribution inside optical material 810 can be modified such that thetemperature of the previously “hot” regions is lowered and laser beam803 can be shifted to those regions while the temperature of thepreviously “cold” region is raised. For example, at time 802 (FIG. 8B),a laser beam can shift from right to left in a differentlower-temperature region of optical material 810 (shown as the topregion). Thus, a time-dependent temperature gradient can be createdinside optical material 810. The cycles shown in FIGS. 8A and 8B can berepeated multiple times.

To illustrate certain aspects of the present invention, an experimentalstudy of the lifetime of Cesium Lithium Borate (CLBO) crystal wasperformed. The wavelength at which the study was performed is 193.3 nm.No bleaching radiation was used and only the temperature of the CLBOcrystal was varied to find an optimum phonon population. The lifetime ofthe crystal was defined as the time it took for the transmission of193.3 nm radiation through the CLBO crystal to decrease by 5%. ThreeCLBO samples grown at different times under different conditions wereanalyzed and the data was combined to obtain average lifetime asfunction of crystal temperature.

FIG. 9 illustrates results of temperature optimization to maximizelifetime of a non-linear CLBO crystal under exposure to 193.3 nmradiation. As shown in FIG. 9, an optimum temperature of −125° C.corresponds to the crystal's maximum lifetime. The lifetime fallssharply on both sides of the optimum temperature. For example, thelifetime at 150° C., which is the temperature at which CLBO crystals aretypically used, was almost half of that at 125° C. The reason for thisbehavior, as explained above is increased transient color centerformation via phonon-assisted absorption due to excessive phononpopulation at high temperatures, while inadequate annealing due toinsufficient number of phonons decreases lifetime at low temperatures.

Although illustrative embodiments of the invention have been describedin detail herein with reference to the accompanying figures, theembodiments described herein are not intended to be exhaustive or tolimit the invention to the precise forms disclosed. As such, manymodifications and variations will be apparent. For example, in oneembodiment, the optical material can be integrally formed as part of thelaser light source. Note that although a CLBO crystal is describedherein, other optical materials that can benefit from suppression oftransient color center formation may include BBO (beta-barium borate),CBO (cesium triborate), LBO (lithium triborate), KDP (potassiumdihydrogen phosphate), KD*P, ADP (ammonium dihydrogen phosphate), KTP(potassium titanyl phosphate), or periodically polled material.Accordingly, it is intended that the scope of the invention be definedby the following Claims and their equivalents.

1. A method for increasing a lifetime of an optical material exposed to a laser light source, the laser light source generating a laser beam having at least one wavelength λ₁, the method comprising: providing a bleaching light source that generates a bleaching light beam having a wavelength λ_(b), wherein λ_(b)>>λ₁; combining the bleaching light beam with the laser beam to generate a combined beam; and using the combined beam for operation of a laser system including the optical material.
 2. The method of claim 1, further including adjusting a temperature of the optical material to provide annealing during the operation of the laser system.
 3. The method of claim 2, wherein the laser light source is pulsed, and wherein the temperature is kept low while laser pulses are present in the optical material, and the temperature is kept high when no laser pulses are present in the optical material.
 4. A method for increasing a lifetime of an optical material exposed to a laser light source, the laser light source generating multiple laser beams having at least one wavelength λ₁, the method comprising: providing a bleaching light source that generates a bleaching light beam having a wavelength λ_(b), wherein λ_(b)>>λ₁; focusing the multiple laser beams at a point in the optical material; intersecting the point with the bleaching light beam; and using the intersected point for operation of a laser system including the optical material.
 5. The method of claim 4, further including adjusting a temperature of the optical material to provide annealing.
 6. The method of claim 5, wherein the laser light source is pulsed, and wherein the temperature is kept low while laser pulses are present in the optical material, and the temperature is kept high when no laser pulses are present in the optical material.
 7. A method for increasing a lifetime of an optical material exposed to a laser light source, the laser light source generating multiple laser beams having at least one wavelength, the method comprising: providing an optical delay element for delaying at least one wavelength of the multiple laser beams; combining a delayed wavelength with any remaining un-delayed wavelengths to generate a combined beam; and using the combined beam for operation of a laser system including the optical material.
 8. The method of claim 7, further including adjusting a temperature of the optical material to provide annealing.
 9. The method of claim 8, wherein the laser light source is pulsed, and wherein the temperature is kept low while laser pulses are present in the optical material, and the temperature is kept high when no laser pulses are present in the optical material.
 10. A method for increasing a lifetime of an optical material exposed to a laser light source, the laser light source generating a laser beam having at least one wavelength, the method comprising: using a bleaching light beam to depopulate a defect energy level inside a band gap of the optical material, the bleaching light beam having a longer wavelength than the laser beam.
 11. The method of claim 10, further including adjusting a temperature of the optical material to provide annealing.
 12. The method of claim 11, wherein the laser light source is pulsed, and wherein the temperature is kept low while laser pulses are present in the optical material, and the temperature is kept high when no laser pulses are present in the optical material.
 13. The method of claim 10, wherein the bleaching light beam propagates parallel to the laser beam.
 14. The method of claim 10, wherein the bleaching light beam propagates at an angle with respect to the laser beam.
 15. The method of claim 10, wherein the laser beam and the bleaching light beam are pulsed, and wherein the pulsed bleaching light beam is time shifted with respect to the pulsed laser beam.
 16. A method for increasing a lifetime of an optical material exposed to a laser light source, the laser light source generating a laser beam having at least one wavelength, the method comprising: delaying one wavelength of the laser beam to bleach at least one defect energy level inside a band gap of the optical material.
 17. A method for increasing a lifetime of an optical material exposed to a laser light source, the method comprising: creating a time-dependent temperature gradient inside the optical material such that a laser beam generated by the laser light source is located inside a region of low temperature in the optical material, wherein the laser beam is shifted through the region.
 18. A laser system comprising: a laser light source for generating a laser beam having at least one wavelength; a bleaching light source for generates a bleaching light beam having a wavelength λ_(b), wherein λ_(b)>>λ₁; and a beam combiner for combining the bleaching light beam with the laser beam to generate a combined beam.
 19. The laser system of claim 18, further including a temperature adjustment component for providing localized annealing.
 20. A laser system comprising: a laser light source for generating multiple laser beams having at least one wavelength; a bleaching light source that generates a bleaching light beam having a wavelength λ_(b), wherein λ_(b)>>λ₁; a focusing lens for focusing the multiple laser beams to a point; and a positioning component for intersecting the point with the bleaching light beam.
 21. The laser system of claim 20, further including a temperature adjustment component for providing localized annealing. 